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A mononuclear iron carbonyl complex [Fe(mu-bdt) (CO)(2)(PTA)(2)] with bulky phosphine ligands: a model for the [FeFe] hydrogenase enzyme active site with an inverted redox potential
- Source :
- Dalton Transactions
- Publication Year :
- 2017
- Publisher :
- ROYAL SOC CHEMISTRY, 2017.
-
Abstract
- A mononuclear hexa-coordinated iron carbonyl complex [Fe(mu-bdt)(CO)(2)(PTA)(2)](1) (bdt = 1,2-benzenedithiolate; PTA = 1,3,5-triaza-7-phosphaadamantane) with two bulky phosphine ligands in the trans position was synthesized and characterized by X-ray structural analysis coulometry data, FTIR, electrochemistry and electronic structure calculations. The complex undergoes a facilitated two-electron reduction 1/1(2-) and shows an inverted one-electron reduction for 1/1(-) at higher potentials. Electrochemical investigations of 1 are compared to the closely related [Fe(bdt)(CO)(2)(PMe3)(2)] compound. A mechanistic suggestion for the hydrogen evolution reaction upon proton reduction from acid media is derived. The stability of 1 in both weak and strong acids is monitored by cyclic voltammetry.
- Subjects :
- Hydrogenase
Proton Reduction
Generation
Electron-Transfer
010402 general chemistry
Photochemistry
Electrochemistry
01 natural sciences
Redox
Functional Models
Inorganic Chemistry
Coulometry
chemistry.chemical_compound
Polymer chemistry
Oxidation
2-Electron Reduction
Fourier transform infrared spectroscopy
biology
010405 organic chemistry
Active site
Pendant Amines
Electrocatalyst
0104 chemical sciences
chemistry
Coordination
biology.protein
Cyclic voltammetry
Phosphine
Subjects
Details
- Language :
- English
- ISSN :
- 23813652
- Database :
- OpenAIRE
- Journal :
- IndraStra Global
- Accession number :
- edsair.doi.dedup.....b5a14922ba458b795a8b16c85578351e